INVESTIGATIONS OF ACTIVE-SITES FOR METHANE ACTIVATION IN THE OXIDATIVE COUPLING REACTION OVER PURE AND LI-PROMOTED MGO CATALYSTS

被引:63
作者
WU, MC [1 ]
TRUONG, CM [1 ]
COULTER, K [1 ]
GOODMAN, DW [1 ]
机构
[1] TEXAS A&M UNIV SYST,DEPT CHEM,COLL STN,TX 77843
关键词
D O I
10.1006/jcat.1993.1089
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The oxidative coupling of methane to ethane over model MgO catalysts prepared under well-controlled, ultrahigh vacuum (UHV) conditions has been studied using a combination of surface science techniques and elevated-pressure kinetic measurements. The utilization of electron energy loss spectroscopy has allowed us to characterize a variety of defects and to identify the active sites which are responsible for the methane coupling reaction. The results indicate that [Li+O-] centers are not likely directly involved in the methane activation step, but rather promote the production of F-type centers in the near-surface region which are responsible for this key step in the methane coupling reaction. The origin of [Li+O-] and F-type defects and their densities and stabilities are discussed. © 1993 Academic Press, Inc.
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页码:344 / 352
页数:9
相关论文
共 32 条
  • [1] ABRAHAM MM, 1976, PHYS REV LETT, V37, P849, DOI 10.1103/PhysRevLett.37.849
  • [2] FORMATION AND STABILITY OF V- AND V A1 CENTERS IN MGO
    ABRAHAM, MM
    CHEN, Y
    UNRUH, WP
    [J]. PHYSICAL REVIEW B, 1974, 9 (04): : 1842 - 1852
  • [3] ANDERSON JR, 1989, APPL CATAL, V47, P177, DOI 10.1016/S0166-9834(00)83227-3
  • [4] OXIDATIVE COUPLING OF METHANE OVER ULTRAFINE CRYSTALLINE MGO DOPED WITH LI - ROLE OF LOWER COORDINATIVE SURFACE SITES PRODUCED BY LI-DOPING
    ANPO, M
    SUNAMOTO, M
    DOI, T
    MATSUURA, I
    [J]. CHEMISTRY LETTERS, 1988, (04) : 701 - 704
  • [5] LOW-ENERGY AUGER TRANSITIONS IN MAGNESIUM-OXIDE
    BERMUDEZ, VM
    RITZ, VH
    [J]. SURFACE SCIENCE, 1979, 82 (02) : L601 - L609
  • [6] VALENCE COMPENSATION OF THERMALLY GENERATED [LI]0 DEFECTS IN MGO
    BOLDU, JL
    ABRAHAM, MM
    CHEN, Y
    [J]. PHYSICAL REVIEW B, 1979, 19 (09): : 4421 - 4426
  • [7] HIGH-TEMPERATURE AND IONIZATION-INDUCED EFFECTS IN LITHIUM-DOPED MGO SINGLE-CRYSTALS
    CHEN, Y
    TOHVER, HT
    NARAYAN, J
    ABRAHAM, MM
    [J]. PHYSICAL REVIEW B, 1977, 16 (12): : 5535 - 5542
  • [8] COULTER K, 1992, CATAL LETT, V6, P191
  • [9] FORMATION OF GAS-PHASE METHYL RADICALS OVER MGO
    DRISCOLL, DJ
    MARTIR, W
    WANG, JX
    LUNSFORD, JH
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1985, 107 (01) : 58 - 63
  • [10] INITIAL OXIDATION OF THE MG(0001) SURFACE, AN ELECTRON-SPECTROSCOPY STUDY
    FLODSTROM, SA
    MARTINSSON, CWB
    [J]. SURFACE SCIENCE, 1982, 118 (03) : 513 - 522